硫自养反硝化燃料电池脱氮除硫及产电性能的实验研究
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摘要
通过建立硫自养反硝化燃料电池,将硫自养反硝化的两个反应过程分开,研究同步脱氮除硫效果以及产电能力.实验结果表明,硫自养反硝化燃料电池阳极室除硫阴极室脱氮是可行的,在试验范围内,硫化物和硝酸盐去除负荷最大分别为0.36kg·m-3·d-1和0.07kg·m-3·d-1,其功率密度最大为144.03mW·m-3.阴极室微生物具有较好的接收电子的能力,当阴极室硝酸盐浓度较低时,硝酸盐易被还原成氮气;当硝酸盐浓度较高时,反应产物以亚硝酸盐为主.阴极室中硝酸盐浓度的改变对阳极室硫化物的去除和燃料电池的产电性能影响较小.外电阻主要影响阴极室硝酸盐的去除而对阳极室中硫化物的去除基本无影响.当外电阻从5Ω增加到2 000Ω时,硝酸盐的去除率从100%降低至61.75%,降低外电阻有利于提高MFC阴极脱氮效果.
In this paper,the sulfide autotrophic denitrification fuel cell was set up and the two reaction processes was separated to study the effect of simultaneous denitrification and desulfurization and the capacity of electricity generation.The results show that simultaneous desulfurization in anode chamber and nitrate removal in cathode chamber is feasible.In this paper,the sulfide and nitrate removal loads were 0.36 kg·m-3·d-1 and 0.07 kg·m-3·d-1,respectively.The maximum power density was 144.03 mW·m-3.Cathode chamber microorganisms have a good ability to receive electrons.When the cathode chamber nitrate concentration is low,nitrate is easily reduced to nitrogen;when the nitrate concentration is higher,the reaction products to nitrite mainly.The removal of the sulfide in the anode chamber and the performance of the fuel cell were less affected by the change of nitrate concentration in the cathode chamber.The external resistance mainly affects the removal of nitrate in the cathode chamber and has no effect on the removal of sulfide in the anode chamber.When the external resistance increases from 5Ωto 2 000Ω,the removal rate of nitrate decreases from 100%to61.75%.Reducing the external resistance is helpful to improve the effect of nitrogen removal in cathode of the MFC.
In this paper,the sulfide autotrophic denitrification fuel cell was set up and the two reaction processes was separated to study the effect of simultaneous denitrification and desulfurization and the capacity of electricity generation.The results show that simultaneous desulfurization in anode chamber and nitrate removal in cathode chamber is feasible.In this paper,the sulfide and nitrate removal loads were 0.36 kg·m-3·d-1 and 0.07 kg·m-3·d-1,respectively.The maximum power density was 144.03 mW·m-3.Cathode chamber microorganisms have a good ability to receive electrons.When the cathode chamber nitrate concentration is low,nitrate is easily reduced to nitrogen;when the nitrate concentration is higher,the reaction products to nitrite mainly.The removal of the sulfide in the anode chamber and the performance of the fuel cell were less affected by the change of nitrate concentration in the cathode chamber.The external resistance mainly affects the removal of nitrate in the cathode chamber and has no effect on the removal of sulfide in the anode chamber.When the external resistance increases from 5Ωto 2 000Ω,the removal rate of nitrate decreases from 100%to61.75%.Reducing the external resistance is helpful to improve the effect of nitrogen removal in cathode of the MFC.
引文
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[24]毛艳萍,蔡兰坤,张乐华,等.微生物燃料电池处理模拟含硫废水的初步研究[J].水处理技术,2010,36(2):105-108.
[25]Liu H,Zhang B,Liu Y,et al.Continuous bioelectricity generation with simultaneous sulfide and organics removals in an anaerobic baffled stacking microbial fuel cell[J].Int.J.Hydrogen Energy,2015,40(25):8 128-8 136.
[26]Jang J K,Pham T H,Chang I S,et al.Construction and operation of a novel mediator-and membrane-less microbial fuel cell[J].Process Biochemistry,2004,39(8):1 007-1 012.
[27]Zhang F,He Z.Simultaneous nitrification and denitrification with electricity generation in dual-cathode microbial fuel cells[J].Chemistry Technology Biotechnology,2012,87(1):153-159.
[28]Cheng S A,Liu H,Logan B E.Increased power generation in a continuous flow MFC with advective flow through the porous anode and reduced electrode spacing[J].Environmental Science Technology,2006(40):2 426-2 432.
[2]Guardia A D,Petiot C,Rogeau D,et al.Influence of aeration rate on nitrogen dynamics during composting[J].Water Management,2008,28(3):575-587.
[3]Sharma K R,Yua Z,Haas D,et al.Dynamics and dynamic modelling of H2S produdtion in sewer systems[J].Water Research,2008,42(10-11):2 527-2 538.
[4]叶建锋.废水生物脱氮处理新技术[M].北京:化学工业出版社,2006.
[5]Young F M,Micklem J,Humpage A R.Effects of bluegreen algal toxin cylindrospermopsin(CYN)on human granulosa cells in vitro[J].Reproductive Toxicology,2008,25(3):374-380.
[6]Lau G N,Sharma K R,Chen G H,et al.Integration of sulfate reduction,autotrophic denitrification and nitrification to achieve low-cost excess sludge minimization for Hong Kong sewage[J].Water Science and Technology,2006,53(3):227-235.
[7]Oh S E,Yoo Y B,Young J C,et al.Effect of organics on sulfur-utilizing autotrophic denitrification under mixotrophic conditions[J].Journal of Biotechnology,2001,92(1):1-8.
[8]张丽,黄勇,袁怡,等.生物同步脱氮除硫工艺研究进展[J].环境污染与防治,2012,34(12):70-73.
[9]Jrgensen B A.Thiosulfate shunt in the sulfur cycle of marine sediments[J].Science,1990,249(4 965):152-154.
[10]王爱杰,杜大钟,任南琪.脱氮硫杆菌同步脱硫反硝化工艺的关键因素研究[J].地球科学进展,2004,19(1):533-536.
[11]Krishnakumar B,Manilal V B.Bacterial oxidation of sulphide under denitrification conditions[J].Biotechnology ietters,1999,21(5):437-440.
[12]An S,Tang K,Nemati M.Simultaneous biodesulphurization and denitrification using an oil reservoir microbial culture:Effects of sulphide loading rate and sulphide to nitrate loading ratio[J].Water Research,2010,44(10):1 531-1 541.
[13]Gadekar S,Nemati M,Hill G A.Batch and continous biooxidation of sulphide by Thiomicrospira sp.CVO:Reaction kinetics and stoichiometry[J].Water Research,2006,40(12):2 436-2 446.
[14]Qaisar M,Zheng P.Anoxic sulfide biooxidation using nitrite as electron acceptor[J].Journal of Hazardous Materials 2007,147(1-2):249-256.
[15]Qaisar M,Zheng P.Effect of pH on anoxic sulfide oxidizing reactor performance[J].Bioresource Technology2008,99(8):3 291-3 296.
[16]蔡靖.同步厌氧脱氮除硫工艺及微生物学特性的研究[D].杭州:浙江大学,2010.
[17]Cai J,Zheng P,Qaisar M.Effect of sulfide to nitrate ratios on the simultaneous anaerobic sulfide and nitrate removal[J].Bioresource Technology,2008,99(13):5 520-5 527.
[18]Cai J,Zheng P.Simultaneous anaerobic sulfide and nitrate removal coupled with electricity generation in microbial fuel cell[J].Biorsource Technology,2013,129(2):224-228.
[19]Cai J,Zheng P.Simultaneous anaerobic sulfide and nitrate removal in microbial fuel cell[J].Biorsource Technology,2013,128(2):760-764.
[20]Sun M,Mu Z X,Chen Y P,et al.Microbe-assisted sulfide oxidation in the anode of a microbial fuel cell[J].Environ.Sci.Technol,2009,43(9):3 372-3 377.
[21]Li W,Zhang S,Chen G,et al.Simultaneous electricity generation and pollutant removal in microbial fuel cell with denitrifying biocathode over nitrite[J].Applied Energy,2014,126(1):136-141.
[22]杨赛风,张建民,崔心水,等.微生物燃料电池阳极氨氮去除的影响因素[J].西安工程大学学报,2016,30(3):284-289.
[23]蔡靖,郑平,胡宝兰,等.硫氮比对厌氧生物同步脱氮除硫工艺性能的影响[J].环境科学学报,2008(8):1 506-1 514.
[24]毛艳萍,蔡兰坤,张乐华,等.微生物燃料电池处理模拟含硫废水的初步研究[J].水处理技术,2010,36(2):105-108.
[25]Liu H,Zhang B,Liu Y,et al.Continuous bioelectricity generation with simultaneous sulfide and organics removals in an anaerobic baffled stacking microbial fuel cell[J].Int.J.Hydrogen Energy,2015,40(25):8 128-8 136.
[26]Jang J K,Pham T H,Chang I S,et al.Construction and operation of a novel mediator-and membrane-less microbial fuel cell[J].Process Biochemistry,2004,39(8):1 007-1 012.
[27]Zhang F,He Z.Simultaneous nitrification and denitrification with electricity generation in dual-cathode microbial fuel cells[J].Chemistry Technology Biotechnology,2012,87(1):153-159.
[28]Cheng S A,Liu H,Logan B E.Increased power generation in a continuous flow MFC with advective flow through the porous anode and reduced electrode spacing[J].Environmental Science Technology,2006(40):2 426-2 432.